Structure and Reactivity of Nanoalloys

Heterogeneous catalysis is key to many large-scale industrial processes and in fostering a sustainable future. In recent years, bimetallic nanoparticles (BiM NPs) have been of great experimental interests in the field of heterogeneous catalysis. Indeed, alloying of metal atoms at the nanoscale often leads to improved catalytic activity, selectivity or resistance to poisoning as compared to monometallic NPs. However, the capability to design novel and more efficient BiM catalysts is presently hampered by the lack of a clear picture of structure-reactivity relationships, resulting in very poor access to reaction mechanisms. As a result, research and development of BiM catalysts still mainly involves laborious trial-and-error processes.
To understand the interplay between surface structuration and catalytic properties of BiM nanocatalysts, the Me-ANS group develops advance TEM studies to access the structural changes undergone by catalysts during reaction with single atom sensitivity. Our approach combines both ex situ post-mortem TEM and recently, in situ gas TEM using high pressure gas cells with unprecedented access to the structural evolution of BiM catalysts “in action” under pressure/temperature conditions close to that encountered during laboratory catalytic testing (i.e. atmospheric pressure and/or at high temperature). Through close collaboration with French/international experts in the synthesis/testing of BiM nanocatalysts and their modeling, our aim is to determine the origins of the promotional effect of metal alloying in bimetallic systems so as to guide the rational design of more active catalysts in different reactions. Systems studied recently in the group include Pd-Au, Pd-Ir and Cu-Au BiM NPs and we are presently investigating the reactivity of high entropy nanoalloys

 
Atomic-scale Operando TEM ! Transformation of a sub-3 nm gold catalyst from a FCC structure to a pseudo-icosaedral morphology driven by the interaction with hydrogen (STEM imaging at atmospheric pressure). Small 17, 2104571 (2021)

Projects :
ANR DINAMIC (2011 – 2014)
ANR TOTEM (2018 – 2021)

Main collaborators :
Laurent Piccolo – Institute of Researches on Catalysis and Environment of Lyon (IRCELYON)
Catherine Louis / Laurent Delannoy – Réactivité de Surface laboratory (Pierre et Marie Curie University).
Hazar Guesmi – Charles Gerhardt Institute, Montpellier
Beien Zhu – Institute of Applied Physics of Shanghai, China

Main publications :

Atomic Scale Observation of the Structural Dynamics of Supported Gold Nanocatalysts under 1,3-Butadiene by in situ Environmental Transmission Electron Microscopy
Abdallah Nassereddine Laurent DelannoyChristian RicolleauCatherine LouisDamien AlloyeauGuillaume WangQing WangHazar GuesmiJaysen Nelayah
ChemCatChem (2023)

Co−Ru Nanoalloy Catalysts for the Acceptorless Dehydrogenation of Alcohols
B. Azeredo, T. Ben Ghzaiel, N. Huang, K. Kaźmierczak, W. Shen, G. Wang, D. Schaming, P. Beaunier, P. Decorse, N. Perret, J. Peron, M. Giraud, C. Michel, L. Sicard and JY. Piquemal
ACS Appl. Nano Mater. 2022, 5, 4, 5733–5744 (2022)

Cu segregation in Au-Cu nanoparticles exposed to hydrogen atmospheric pressure : how is fcc symmetry maintained ?
Q. Wang, A. Nassereddine, D. Loffreda, C. Ricolleau, D. Alloyeau, C. Louis, L. Delannoy, J. Nelayah and H. Guesmi
Faraday Discussions just accepted (2022)

Revealing Size Dependent Structural Transitions in Supported Gold Nanoparticles in Hydrogen at Atmospheric Pressure
A. Nassereddine, Q. Wang, D. Loffreda, C. Ricolleau, D. Alloyeau, C. Louis, L. Delannoy, J. Nelayah and H. Guesmi
Small 17, 2104571 (2021)

Reshaping Dynamics of Gold Nanoparticles under H2 and O2 at Atmospheric Pressure
Adrian Chmielewski, Jun Meng, Beien Zhu, Yi Gao, Hazar Guesmi, Hélène Prunier, Damien Alloyeau, Guillaume Wang, Catherine Louis, Laurent Delannoy, Pavel Afanasiev, Christian Ricolleau, Jaysen Nelayah
ACS Nano 13, 2024-2033 (2019)

On the Influence of Oxygen On the Degradation of Fe‐N‐C Catalysts
Kavita Kumar, Laetitia Dubau, Michel Mermoux, Jingkun Li, Andrea Zitolo, Jaysen Nelayah, Frederic Jaouen, Frederic Maillard
Angewandte Chemie 2019

Nanoscale temperature measurement during temperature controlled in situ TEM using Al plasmon nanothermometry
A Chmielewski, C Ricolleau, D Alloyeau, G Wang, J Nelayah
Ultramicroscopy 209, 112881 (2019)

Nanostructured Nickel Aluminate as a Key Intermediate for the Production of Highly Dispersed and Stable Nickel Nanoparticles Supported within Mesoporous Alumina for Dry Reforming of Methane
Leila Karam, Julien Reboul, Nissrine El Hassan, Jaysen Nelayah, Pascale Massiani
Molecules 2019, 24(22), 4107

Selective hydrogenation of butadiene over TiO2 supported copper, gold and gold–copper catalysts prepared by deposition–precipitation
Laurent Delannoy, Gode Thrimurthulu, Padigapati S Reddy, Christophe Méthivier, Jaysen Nelayah, Benjaram M Reddy, Christian Ricolleau, Catherine Louis
Phys. Chem. Chem. Phys. 16 (48), 26514-26527

Long-range chemical orders in Au–Pd nanoparticles revealed by aberration-corrected electron microscopy
J Nelayah, NT Nguyen, D Alloyeau, GY Wang, C Ricolleau
Nanoscale 6 (17), 10423-10430

Nanoalloying bulk-immiscible iridium and palladium inhibits hydride formation and promotes catalytic performances
C Zlotea, F Morfin, TS Nguyen, NT Nguyen, J Nelayah, C Ricolleau, M Latroche, L Piccolo
Nanoscale 6 (17), 9955-9959

Au–Rh and Au–Pd nanocatalysts supported on rutile titania nanorods : structure and chemical stability
Zere Konuspayeva, Pavel Afanasiev, Thanh-Son Nguyen, Luca Di Felice, Franck Morfin, Nhat-Tai Nguyen, Jaysen Nelayah, Christian Ricolleau, Z. Y. Li, Jun Yuan, Gilles Berhault and Laurent Piccolo
Phys. Chem. Chem. Phys. (2015)

New insights into the mixing of gold and copper in a nanoparticle from a structural study of Au–Cu nanoalloys synthesized via a wet chemistry method and pulsed laser deposition
Hélène Prunier, Jaysen Nelayah, Christian Ricolleau, Guillaume Wang, Sophie Nowak, Anne-Félicie Lamic-Humblot and Damien Alloyeau
Phys. Chem. Chem. Phys. (2015)

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